Abstract: Single indole alkaloids(containing vindoline and catharanthine) and double indole alkaloids (containing vinblastine) were separated from the total alkaloids of Catharanthus roseus by pH gradient extraction according to their different existing statuses under different pH values. The single indole alkaloids part was further isolated by alkaline aluminum oxide column chromatography. After the process of pH gradient extraction，the contents of vindoline and catharanthine are 18.12% and 11.44%，respectively，and their recoveries are 80.86% and 88.91%，respectively. After alkaline aluminum oxide column chromatography，the contents of vindoline and catharanthine are 85.56% and 76.73%，respectively，and their recoveries are 85.23% and 86.34%，respectively. After recrystallization，the contents of vindoline and catharanthine are 95.22% and 98.46%，and their recoveries are 92.15% and 98.24%, respectively. This process is suitable for large-scale industrial production of vindoline and catharanthine.